On the Conformation of Dimeric Acceptors and Their Polymer Solar Cells with Efficiency over 18 .

The determination of molecular conformations of oligomeric acceptors (OAs) and their impact on molecular packing are crucial for understanding the photovoltaic performance of their resulting polymer solar cells (PSCs) but have not been well studied yet. Herein, we synthesized two dimeric acceptor materials, DIBP3F-Se and DIBP3F-S, which bridged two segments of Y6-derivatives by selenophene and thiophene, respectively. Theoretical simulation and experimental 1D and 2D NMR spectroscopic studies prove that both dimers exhibit O-shaped conformations other than S- or U-shaped counter-ones. Notably, this O-shaped conformation is likely governed by a distinctive "conformational lock" mechanism, arising from the intensified intramolecular π-π interactions among their two terminal groups within the dimers. PSCs based on DIBP3F-Se deliver a maximum efficiency of 18.09 %, outperforming DIBP3F-S-based cells (16.11 %) and ranking among the highest efficiencies for OA-based PSCs. This work demonstrates a facile method to obtain OA conformations and highlights the potential of dimeric acceptors for high-performance PSCs.

Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx.

The performance of perovskite solar cells with inverted polarity (p-i-n) is still limited by recombination at their electron extraction interface, which also lowers the power conversion efficiency (PCE) of p-i-n perovskite-silicon tandem solar cells. A MgFx interlayer with thickness of ~1 nanometer at the perovskite/C60 interface favorably adjusts the surface energy of the perovskite layer through thermal evaporation, which facilitates efficient electron extraction and displaces C60 from the perovskite surface to mitigate nonradiative recombination. These effects enable a champion open-circuit voltage of 1.92 volts, an improved fill factor of 80.7%, and an independently certified stabilized PCE of 29.3% for a monolithic perovskite-silicon tandem solar cell ~1 square centimeter in area. The tandem retained ~95% of its initial performance after damp-heat testing (85°C at 85% relative humidity) for >1000 hours.

Probing Ultrafast Interfacial Carrier Dynamics in Metal Halide Perovskite Films and Devices by Transient Reflection Spectroscopy.

Interfaces in metal halide perovskite (MHP) solar cells cause carrier recombination and thereby reduce their power conversion efficiency. Here, ultrafast (picosecond to nanosecond) transient reflection (TR) spectroscopy has been used to probe interfacial carrier dynamics in thin films of the reference MHP MAPbI3 and state-of-the-art (Cs0.15MA0.15FA0.70)Pb(Br0.20I0.80)3 (CsFAMA). First, MAPbI3 films in contact with fullerene-based charge extraction layers (CTLs) in the presence and absence of LiF used as an interlayer (ITL) were studied. To quantify and discriminate between interface-induced and bulk carrier recombination, we employed a one-dimensional diffusion and recombination model. The interface-induced carrier recombination velocity was found to be 1229 ± 78 cm s-1 in nonpassivated MAPbI3 films, which was increased to 2248 ± 75 cm s-1 when MAPbI3 interfaced directly with C60, whereas it was reduced to 145 ± 63 cm s-1 when inserting a 1 nm thin LiF interlayer between MAPbI3 and C60, in turn improving the open-circuit voltage of devices by 33 mV. Second, the effect of surface and grain boundary passivation by PhenHCl in CsFAMA was revealed. Here, the recombination velocity decreased from 605 ± 52 to 0.16 ± 5.28 and 7.294 ± 34.5 cm s-1, respectively. The approach and data analysis presented here are immediately applicable to other perovskite/interlayer/CTL interfaces and passivation protocols, and they add to our understanding of the impact of surfaces and interfaces in MHP-based thin films on carrier recombination and device efficiency.

Tin Oxide Electron-Selective Layers for Efficient, Stable, and Scalable Perovskite Solar Cells.

Perovskite solar cells (PSCs) have become a promising photovoltaic (PV) technology, where the evolution of the electron-selective layers (ESLs), an integral part of any PV device, has played a distinctive role to their progress. To date, the mesoporous titanium dioxide (TiO2 )/compact TiO2 stack has been among the most used ESLs in state-of-the-art PSCs. However, this material requires high-temperature sintering and may induce hysteresis under operational conditions, raising concerns about its use toward commercialization. Recently, tin oxide (SnO2 ) has emerged as an attractive alternative ESL, thanks to its wide bandgap, high optical transmission, high carrier mobility, suitable band alignment with perovskites, and decent chemical stability. Additionally, its low-temperature processability enables compatibility with temperature-sensitive substrates, and thus flexible devices and tandem solar cells. Here, the notable developments of SnO2 as a perovskite-relevant ESL are reviewed with emphasis placed on the various fabrication methods and interfacial passivation routes toward champion solar cells with high stability. Further, a techno-economic analysis of SnO2 materials for large-scale deployment, together with a processing-toxicology assessment, is presented. Finally, a perspective on how SnO2 materials can be instrumental in successful large-scale module and perovskite-based tandem solar cell manufacturing is provided.

Lewis-Acid Doping of Triphenylamine-Based Hole Transport Materials Improves the Performance and Stability of Perovskite Solar Cells.

Highly efficient perovskite solar cells (PSCs) fabricated in the classic n-i-p configuration generally employ triphenylamine-based hole-transport layers (HTLs) such as spiro-OMeTAD, PTAA, and poly-TPD. Controllable doping of such layers has been critical to achieve increased conductivity and high device performance. To this end, LiTFSI/tBP doping and subsequent air exposure is widely utilized. However, this approach often leads to low device stability and reproducibility. Departing from this point, we introduce the Lewis acid tris(pentafluorophenyl)borane (TPFB) as an effective dopant, resulting in a significantly improved conductivity and lowered surface potential for triphenylamine-based HTLs. Here, we specifically investigated spiro-OMeTAD, which is the most widely used HTL for n-i-p devices, and revealed improved power conversion efficiency (PCE) and stability of the PSCs. Further, we demonstrated the applicability of TPFB doping to other triphenylamine-based HTLs. Spectroscopic characterizations reveal that TPFB doping results in significantly improved charge transport and reduced recombination losses. Importantly, the TPFB-doped perovskite devices retained near 85% of the initial PCE after 1000 h of storage in the air, while the conventional LiTFSI-doped device dropped to 75%. Finally, we give insight into utilizing other similar molecular dopants such as fluorine-free triphenylborane and phosphorus-centered tris(pentafluorophenyl)phosphine (TPFP) by density functional theory analysis underscoring the significance of the central boron atom and fluorination in TPFB for the formation of Lewis acid-base adducts.

Efficient tandem solar cells with solution-processed perovskite on textured crystalline silicon.

Stacking solar cells with decreasing band gaps to form tandems presents the possibility of overcoming the single-junction Shockley-Queisser limit in photovoltaics. The rapid development of solution-processed perovskites has brought perovskite single-junction efficiencies >20%. However, this process has yet to enable monolithic integration with industry-relevant textured crystalline silicon solar cells. We report tandems that combine solution-processed micrometer-thick perovskite top cells with fully textured silicon heterojunction bottom cells. To overcome the charge-collection challenges in micrometer-thick perovskites, we enhanced threefold the depletion width at the bases of silicon pyramids. Moreover, by anchoring a self-limiting passivant (1-butanethiol) on the perovskite surfaces, we enhanced the diffusion length and further suppressed phase segregation. These combined enhancements enabled an independently certified power conversion efficiency of 25.7% for perovskite-silicon tandem solar cells. These devices exhibited negligible performance loss after a 400-hour thermal stability test at 85°C and also after 400 hours under maximum power point tracking at 40°C.

The Effect of Methylammonium Iodide on the Supersaturation and Interfacial Energy of the Crystallization of Methylammonium Lead Triiodide Single Crystals.

It is very important to study the crystallization of hybrid organic-inorganic perovskites because their thin films are usually prepared from solution. The investigation on the growth of perovskite films is however limited by their polycrystallinity. In this work, methylammonium lead triiodide single crystals grown from solutions with different methylammonium iodide (MAI):lead iodide (PbI2 ) ratios were investigated. We observed a V-shaped dependence of the crystallization onset temperature on the MAI:PbI2 ratio. This is attributed to the MAI effects on the supersaturation of precursors and the interfacial energy of the crystal growth. At low MAI:PbI2 ratio (<1.7), more MAI leads to the supersaturation of the precursors at lower temperature. At high MAI:PbI2 ratio, the crystal growing plans change from (100)-plane dominated to (001)-plane dominated. The latter have higher interfacial energy than the former, leading to a higher crystallization onset temperature.

Factors Influencing the Mechanical Properties of Formamidinium Lead Halides and Related Hybrid Perovskites.

The mechanical properties of formamidinium lead halide perovskites (FAPbX3 , X=Br or I) grown by inverse-temperature crystallization have been studied by nanoindentation. The measured Young's moduli (9.7-12.3 GPa) and hardnesses (0.36-0.45 GPa) indicate good mechanical flexibility and ductility. The effects of hydrogen bonding were evaluated by performing ab initio molecular dynamics on both formamidinium and methylammonium perovskites and calculating radial distribution functions. The structural and chemical factors influencing these properties are discussed by comparison with corresponding values in the literature for other hybrid perovskites, including double perovskites. Our results reveal that bonding in the inorganic framework and hydrogen bonding play important roles in determining elastic stiffness. The influence of the organic cation becomes more important for structures at the limit of their perovskite stability, indicated by high tolerance factors.